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Abstract The phase transitions in MnNiGe compounds were explored by manipulating the heat treatment conditions and through hydrostatic pressure application. As the quenching temperature increased, both the first-order martensitic structural transition temperatures and magnetic transition temperatures decreased relative to those in the slowly-cooled samples. When the samples were quenched from 1200 ^∘C, the first-order martensitic structural transition temperature lowered by more than 200 K. The structural transitions also shifted to lower temperature with the application of hydrostatic pressure during measurement. Temperature-dependent x-ray diffraction results reveal that the changes of the cell parameters resulting from the structural transitions are nearly identical for all samples regardless of the extensive variation in their structural transition temperatures. In addition, neutron scattering measurements confirm the magnetic structure transition between simple and cycloidal spiral magnetic structures. 

The effects of doping, hydrostatic pressure, and thermal quenching on the phase transitions and magnetocaloric properties of the Mn1−xCoxNiGe system have been investigated. Cobalt doping on the Mn site shifted the martensitic structural transition toward lower temperature until it was ultimately absent, leaving only a magnetic transition from a ferromagnetic (FM) to a paramagnetic (PM) state in the high-temperature hexagonal phase. Co-occurrence of the magnetic and structural transitions to form a first-order magnetostructural transition (MST) from the FM orthorhombic to the PM hexagonal phase was observed in samples with 0.05 < x < 0.20. An additional antiferromagnetic–ferromagnetic-like transition was observed in the martensite phase for 0.05 < x < 0.10, which gradually vanished with increasing Co concentration (x > 0.10) or magnetic field (H > 0.5 T). The application of external hydrostatic pressure shifted the structural transition to lower temperature until an MST was formed in samples with x = 0.03 and 0.05, inducing large magnetic entropy changes up to −80.3 J kg−1 K−1 (x = 0.03) for a 7-T field change under 10.6-kbar pressure. Similar to the effects of the application of hydrostatic pressure, an MST was formed near room temperature in the sample with x = 0.03 by annealing at high temperature (1200 °C) followed by quenching, resulting in a large magnetic entropy change of −56.2 J kg−1 K−1. These experimental results show that the application of pressure and thermal quenching, in addition to compositional variations, are effective methods to create magnetostructural transitions in the MnNiGe system, resulting in large magnetocaloric effects. 

Metastable phases were formed in Mn1−xCoxNiGe (x=0.05 and 0.08) by annealing at 800 °C followed by rapid cooling, i.e., quenching, at ambient pressure (P=0) and under a pressure of P=3.5 GPa, and their phase transitions and associated magnetocaloric properties were investigated. The crystal cell volumes of the metastable phases decreased, and their structural transitions significantly shifted to lower temperatures relative to those of the slow-cooled compounds, with a greater reduction observed in the samples where the rapid cooling occurred under high pressures. The magnetic and structural transitions coupled to form a magnetostructural transition in the metastable phases, resulting in large magnetic entropy changes up to −79.6 J kg−1 K−1 (x=0.08) for a 7-T field change. The experimental results demonstrate thermal quenching and high-pressure annealing as alternative methods to create magnetostructural transitions, without modifying the compositions of the materials.